Carbon Defect Characterization of Nitrogen-Doped Reduced Graphene Oxide Electrocatalysts for the Two-Electron Oxygen Reduction Reaction
Abstract
© 2019 American Chemical Society. Numerous modified-carbon catalysts have been developed for the direct synthesis of hydrogen peroxide through electrochemical oxygen reduction. However, given the complex structure of most porous carbons and the poor oxygen reduction reaction (ORR) selectivity typically observed when they are used as catalysts, it is still unclear which carbon defects are responsible for the high two-electron ORR activity typically observed in these materials. Here, we study electrocatalytic peroxide formation activity of nitrogen-doped reduced graphene oxide (N-rGO) materials to relate carbon defects to electrocatalytic activity. To do so, we selected two N-rGO electrodes that selectively produce peroxide at all potentials studied (0.70-0.10 V vs RHE) under alkaline conditions. Oxygen reduction studies, combined with material characterization, especially solid-state 13carbon nuclear magnetic resonance coupled with magic angle spinning and cross-polarization, demonstrate that epoxy or ether groups in the N-rGO catalyst are likely associated with the active sites that form peroxide at the lowest overpotential in alkaline media.
- Authors:
-
[1];
[3];
[4];
[6];
[7];
[2];
[2];
[8]
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Hanyang Univ., Seoul (Korea, Republic of)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Korea Research Inst. of Chemical Technology, Daejeon (Korea, Republic of)
- Univ. of Texas, Austin, TX (United States)
- Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Santa Cruz, CA (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
- OSTI Identifier:
- 1547070
- Alternate Identifier(s):
- OSTI ID: 1656517
- Grant/Contract Number:
- AC02-76SF00515; 2017R1A2B4010771; 2016R1A6A3A03012382; 2014M1A8A1049307; CBET-1604927; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 31; Journal Issue: 11; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Kim, Hyo Won, Park, Hun, Roh, Ji Soo, Shin, Jae Eun, Lee, Tae Hoon, Zhang, Liang, Cho, Young Hoon, Yoon, Hee Wook, Bukas, Vanessa J., Guo, Jinghua, Park, Ho Bum, Han, Tae Hee, and McCloskey, Bryan D. Carbon Defect Characterization of Nitrogen-Doped Reduced Graphene Oxide Electrocatalysts for the Two-Electron Oxygen Reduction Reaction. United States: N. p., 2019.
Web. doi:10.1021/acs.chemmater.9b00210.
Kim, Hyo Won, Park, Hun, Roh, Ji Soo, Shin, Jae Eun, Lee, Tae Hoon, Zhang, Liang, Cho, Young Hoon, Yoon, Hee Wook, Bukas, Vanessa J., Guo, Jinghua, Park, Ho Bum, Han, Tae Hee, & McCloskey, Bryan D. Carbon Defect Characterization of Nitrogen-Doped Reduced Graphene Oxide Electrocatalysts for the Two-Electron Oxygen Reduction Reaction. United States. https://doi.org/10.1021/acs.chemmater.9b00210
Kim, Hyo Won, Park, Hun, Roh, Ji Soo, Shin, Jae Eun, Lee, Tae Hoon, Zhang, Liang, Cho, Young Hoon, Yoon, Hee Wook, Bukas, Vanessa J., Guo, Jinghua, Park, Ho Bum, Han, Tae Hee, and McCloskey, Bryan D. Wed .
"Carbon Defect Characterization of Nitrogen-Doped Reduced Graphene Oxide Electrocatalysts for the Two-Electron Oxygen Reduction Reaction". United States. https://doi.org/10.1021/acs.chemmater.9b00210. https://www.osti.gov/servlets/purl/1547070.
@article{osti_1547070,
title = {Carbon Defect Characterization of Nitrogen-Doped Reduced Graphene Oxide Electrocatalysts for the Two-Electron Oxygen Reduction Reaction},
author = {Kim, Hyo Won and Park, Hun and Roh, Ji Soo and Shin, Jae Eun and Lee, Tae Hoon and Zhang, Liang and Cho, Young Hoon and Yoon, Hee Wook and Bukas, Vanessa J. and Guo, Jinghua and Park, Ho Bum and Han, Tae Hee and McCloskey, Bryan D.},
abstractNote = {© 2019 American Chemical Society. Numerous modified-carbon catalysts have been developed for the direct synthesis of hydrogen peroxide through electrochemical oxygen reduction. However, given the complex structure of most porous carbons and the poor oxygen reduction reaction (ORR) selectivity typically observed when they are used as catalysts, it is still unclear which carbon defects are responsible for the high two-electron ORR activity typically observed in these materials. Here, we study electrocatalytic peroxide formation activity of nitrogen-doped reduced graphene oxide (N-rGO) materials to relate carbon defects to electrocatalytic activity. To do so, we selected two N-rGO electrodes that selectively produce peroxide at all potentials studied (0.70-0.10 V vs RHE) under alkaline conditions. Oxygen reduction studies, combined with material characterization, especially solid-state 13carbon nuclear magnetic resonance coupled with magic angle spinning and cross-polarization, demonstrate that epoxy or ether groups in the N-rGO catalyst are likely associated with the active sites that form peroxide at the lowest overpotential in alkaline media.},
doi = {10.1021/acs.chemmater.9b00210},
journal = {Chemistry of Materials},
number = 11,
volume = 31,
place = {United States},
year = {Wed May 29 00:00:00 EDT 2019},
month = {Wed May 29 00:00:00 EDT 2019}
}
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